Poly(vinylidene
fluoride) (PVDF) is widely used as a ferroelectric
polymer due to its good flexibility and stability. However, its ferroelectricity
requires enhancement through doping or modification processes, and
the necessity for prepoling significantly limits its applications.
In the present work, we propose an interfacial ion-dipole induction
method for preparing high-ferroelectric PVDF films using oppositely
charged single-chain Janus nanoparticles (OC-SJNPs). The SJNPs possess
a positive end with quaternized amino groups that allow for uniform
electrodeposition on the substrate surface. After hydrolysis, due
to the nanoscale size, proton transfer occurs between carboxyl and
amino groups, thus promoting the degree of ionization and the charge
density of both ends. The negatively charged (−45 mV) end of
OC-SJNPs exhibits strong dipole interaction with PVDF chains, leading
to a high β-phase content of 90.8%, with a residual polarization
strength of 10.6 μC/cm2, nearing the theoretical
maximum of pure PVDF films. Additionally, the orientation of OC-SJNPs
induces the alignment of PVDF dipoles, thus achieving high piezoelectric
energy generation without prepoling. Another polar polymer, polyacrylonitrile
(PAN) also demonstrated higher piezoelectric energy generation by
using the proposed method. It not only successfully prepared high-ferroelectric
and poling-free PVDF films as piezoelectric energy generators but
also offers a universal and efficient approach for the preparation
of polar polymer materials.